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ethylene-co-vinyl alcohol) molecular weight and vinyl alcohol content on morphology, antifouling, and permeationproperties of polysulfone ultrafiltration membrane: thermodynamic and formation hydrodynamic behavior

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1484-1502 doi: 10.1007/s11705-023-2331-y

摘要： Various hydrophilic poly(ethylene-co-vinyl alcohol) (EVOH) were used herein to precisely control the structure and hydrodynamic properties of polysulfone (PSF) membranes. Particularly, to prepare pristine PSF and PSF/EVOH blends with increasing vinyl alcohol (VOH: 73%, 68%, 56%), the non-solvent-induced phase separation (NIPS) technique was used. Polyethylene glycol was used as a compatibilizer and as a porogen in N,N-dimethylacetamide. Rheological and ultrasonic separation kinetic measurements were also carried out to develop an ultrafiltration membrane mechanism. The extracted membrane properties and filtration capabilities were systematically compared to the proposed mechanism. Accordingly, the addition of EVOH led to an increase in the rheology of the dopes. The resulting membranes exhibited a microporous structure, while the finger-like structures became more evident with increasing VOH content. The PSF/EVOH behavior was changed from immediate to delayed segregation due to a change in the hydrodynamic kinetics. Interestingly, the PSF/EVOH32 membranes showed high hydrophilicity and achieved a pure water permeability of 264 L·m–2·h–1·bar–1, which was higher than that of pure PSF membranes (171 L·m–2·h–1·bar–1). In addition, PSF/EVOH32 rejected bovine serum albumin at a high rate (> 90%) and achieved a significant restoration of permeability. Finally, from the thermodynamic and hydrodynamic results, valuable insights into the selection of hydrophilic copolymers were provided to tailor the membrane structure while improving both the permeability and antifouling performance.

关键词： polysulfone     blend modification     ultrafiltration membrane     formation hydrodynamics     poly(ethylene-co-vinyl alcohol) copolymer    

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A CO and CO

Guoxing Chen, Marc Widenmeyer, Binjie Tang, Louise Kaeswurm, Ling Wang, Armin Feldhoff, Anke Weidenkaff

《化学科学与工程前沿（英文）》 2020年 第14卷 第3期   页码 405-414 doi: 10.1007/s11705-019-1886-0

摘要： A series of novel dense mixed conducting ceramic membranes based on K NiF -type (La Ca ) (Ni Cu )O was successfully prepared through a sol-gel route. Their chemical compatibility, oxygen permeability, CO and CO tolerance, and long-term CO resistance regarding phase composition and crystal structure at different atmospheres were studied. The results show that higher Ca contents in the material lead to the formation of CaCO . A constant oxygen permeation flux of about 0.63 mL·min ·cm at 1173 K through a 0.65 mm thick membrane was measured for (La Ca ) (Ni Cu )O , using either helium or pure CO as sweep gas. Steady oxygen fluxes with no sign of deterioration of this membrane were observed with increasing CO concentration. The membrane showed excellent chemical stability towards CO for more than 1360 h and phase stability in presence of CO for 4 h at high temperature. In addition, this membrane did not deteriorate in a high-energy CO plasma. The present work demonstrates that this (La Ca ) (Ni Cu )O membrane is a promising chemically robust candidate for oxygen separation applications.

关键词： K2NiF4 structure     oxygen permeation membrane     CO2 and CO resistances     CO2 plasma resistance     long-term robustness    

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Highly active and durable Pd-Cu catalysts for oxygen reduction in alkaline exchange membrane fuel cells

Xiong PENG, Travis J. OMASTA, Justin M. ROLLER, William E. MUSTAIN

《能源前沿（英文）》 2017年 第11卷 第3期   页码 299-309 doi: 10.1007/s11708-017-0495-1

摘要： A Pd-Cu catalyst, with primary B2-type phase, supported by VulcanXC-7R carbon was synthesized via a solvothermal method. The catalysts were physically and electrochemically characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and both cyclic and linear sweep voltammetry using a rotating disk electrode (RDE). During the RDE testing, the half-wave potential of the Pd-Cu/Vulcan catalyst was 50 mV higher compared to that of commercial Pt/C catalyst for the oxygen reduction reaction (ORR) in alkaline media. The Pd-Cu/Vulcan exhibited a specific activity of 1.27 mA/cm and a mass activity of 0.59 A/mg at 0.9 V, which were 4 and 3 times greater than that of the commercial Pt/C catalyst, respectively. The Pd-Cu/Vulcan catalyst also showed higher alkaline exchange membrane fuel cell (AEMFC) performance, with operating power densities of 1100 MW/cm operating on H /O and 700 MW/cm operating on H /Air (CO -free), which were markedly higher than those of the commercial Pt/C. The Pd-Cu/Vulcan catalyst also exhibited high stability during a short-term, AEMFC durability test, with only around 11% performance loss after 30 hours of operation, an improvement over most AEMFCs reported in the literature to date.

关键词： alkaline exchange membrane (AEM)     fuel cell     Pd-Cu     oxygen reduction     high performance     water    

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Theoretical study on Janus graphene oxide membrane for water transport

Quan Liu, Mingqiang Chen, Yangyang Mao, Gongping Liu

《化学科学与工程前沿（英文）》 2021年 第15卷 第4期   页码 913-921 doi: 10.1007/s11705-020-1954-5

摘要： Graphene oxide (GO) membranes have received considerable attention owing to their outstanding water-permeation properties; however, the effect of the membrane’s microstructures (such as the distribution of oxidized and pristine regions) on the transport mechanism remains unclear. In this study, we performed molecular simulations to explore the permeation of a water–ethanol mixture using a new type of Janus GO membranes with different orientations of oxidized and pristine surfaces. The results indicate that the oxidized upper surface endows the GO membrane with considerable water-capture capability and the in-built oxidized interlayer promotes the effective vertical diffusion of water molecules. Consequently, using the optimized Janus GO membrane, infinite water selectivity and outstanding water flux (~40.9 kg⋅m ⋅h ) were achieved. This study contributes to explaining the role of oxidized regions in water permeation via GO membranes and suggests that Janus GO membranes could be used as potential candidates for water–ethanol separation.

关键词： graphene oxide membrane     molecular dynamics simulation     water permeation     water-ethanol separation     oxidized and pristine regions    

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Effect of PEG additives on properties and morphologies of polyetherimide membranes prepared by phase inversion

Jian CHEN, Jiding LI, Xia ZHAN, Xiaolong HAN, Cuixian CHEN,

《化学科学与工程前沿（英文）》 2010年 第4卷 第3期   页码 300-306 doi: 10.1007/s11705-009-0280-8

摘要： This study investigated the effect of poly(ethylene glycol) (PEG) additive as a pore-former on the structure formation of membranes and their permeation properties connected with the changes in thermodynamic and kinetic properties in the phase inversion process. The membranes were prepared by using polyetherimide/-methyl-2-pyrrolidone/PEG (PEI/NMP/PEG) casting solution and water coagulant. The resulting membranes, prepared by changing the ratio of PEG to PEI, were characterized by scanning electron microscope (SEM) observations, measurements of water flux and -globin rejection. The thermodynamic and kinetic properties of the membrane-forming system were studied through viscosity. The pore radius distribution curves were especially obtained by differential scanning calorimetry (DSC). Furthermore, the membranes were characterized for pure water flux and rejection of solute and by SEM observation. The filtration results agreed well with the SEM observations. As expected, PEG with a fixed molecular weight (PEG 600) acted as a pore forming agent, and membrane porosity increased as the PEG content of the casting solution increased.

关键词： permeation     ethylene     filtration     PEI/NMP/PEG     membrane    

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Exploration of the oxygen transport behavior in non-precious metal catalyst-based cathode catalyst layerfor proton exchange membrane fuel cells

Shiqu CHEN, Silei XIANG, Zehao TAN, Huiyuan LI, Xiaohui YAN, Jiewei YIN, Shuiyun SHEN, Junliang ZHANG

《能源前沿（英文）》 2023年 第17卷 第1期   页码 123-133 doi: 10.1007/s11708-022-0849-1

摘要： High cost has undoubtedly become the biggest obstacle to the commercialization of proton exchange membrane fuel cells (PEMFCs), in which Pt-based catalysts employed in the cathodic catalyst layer (CCL) account for the major portion of the cost. Although non-precious metal catalysts (NPMCs) show appreciable activity and stability in the oxygen reduction reaction (ORR), the performance of fuel cells based on NPMCs remains unsatisfactory compared to those using Pt-based CCL. Therefore, most studies on NPMC-based fuel cells focus on developing highly active catalysts rather than facilitating oxygen transport. In this work, the oxygen transport behavior in CCLs based on highly active Fe-N-C catalysts is comprehensively explored through the elaborate design of two types of membrane electrode structures, one containing low-Pt-based CCL and NPMC-based dummy catalyst layer (DCL) and the other containing only the NPMC-based CCL. Using Zn-N-C based DCLs of different thickness, the bulk oxygen transport resistance at the unit thickness in NPMC-based CCL was quantified via the limiting current method combined with linear fitting analysis. Then, the local and bulk resistances in NPMC-based CCLs were quantified via the limiting current method and scanning electron microscopy, respectively. Results show that the ratios of local and bulk oxygen transport resistances in NPMC-based CCL are 80% and 20%, respectively, and that an enhancement of local oxygen transport is critical to greatly improve the performance of NPMC-based PEMFCs. Furthermore, the activity of active sites per unit in NPMC-based CCLs was determined to be lower than that in the Pt-based CCL, thus explaining worse cell performance of NPMC-based membrane electrode assemblys (MEAs). It is believed that the development of NPMC-based PEMFCs should proceed not only through the design of catalysts with higher activity but also through the improvement of oxygen transport in the CCL.

关键词： proton exchange membrane fuel cells (PEMFCs)     non-precious metal catalyst (NPMC)     cathode catalyst layer (CCL)     local and bulk oxygen transport resistance    

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TiO supported IrO for anode reversal tolerance in proton exchange membrane fuel cell

《能源前沿（英文）》 2022年 第16卷 第5期   页码 852-861 doi: 10.1007/s11708-021-0811-7

摘要： Fuel starvation can occur and cause damage to the cell when proton exchange membrane fuel cells operate under complex working conditions. In this case, carbon corrosion occurs. Oxygen evolution reaction (OER) catalysts can alleviate carbon corrosion by introducing water electrolysis at a lower potential at the anode in fuel shortage. The mixture of hydrogen oxidation reaction (HOR) and unsupported OER catalyst not only reduces the electrolysis efficiency, but also influences the initial performance of the fuel cell. Herein, Ti4O7 supported IrOx is synthesized by utilizing the surfactant-assistant method and serves as reversal tolerant components in the anode. When the cell reverse time is less than 100 min, the cell voltage of the MEA added with IrOx/Ti4O7 has almost no attenuation. Besides, the MEA has a longer reversal time (530 min) than IrOx (75 min), showing an excellent reversal tolerance. The results of electron microscopy spectroscopy show that IrOx particles have a good dispersity on the surface of Ti4O7 and IrOx/Ti4O7 particles are uniformly dispersed on the anode catalytic layer. After the stability test, the Ti4O7 support has little decay, demonstrating a high electrochemical stability. IrOx/Ti4O7 with a high dispersity has a great potential to the application on the reversal tolerance anode of the fuel cell.

关键词： proton exchange membrane fuel cell (PEMFC)     fuel starvation     cell reverse     reversal tolerance anode     oxygen evolution reaction    

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Thermal annealing synthesis of double-shell truncated octahedral Pt-Ni alloys for oxygen reduction reactionof polymer electrolyte membrane fuel cells

Xiashuang LUO, Yangge GUO, Hongru ZHOU, Huan REN, Shuiyun SHEN, Guanghua WEI, Junliang ZHANG

《能源前沿（英文）》 2020年 第14卷 第4期   页码 767-777 doi: 10.1007/s11708-020-0667-2

摘要： Shape-controlled Pt-Ni alloys usually offer an exceptional electrocatalytic activity toward the oxygen reduction reaction (ORR) of polymer electrolyte membrane fuel cells (PEMFCs), whose tricks lie in well-designed structures and surface morphologies. In this paper, a novel synthesis of truncated octahedral PtNi alloy catalysts that consist of homogeneous Pt-Ni alloy cores enclosed by NiO-Pt double shells through thermally annealing defective heterogeneous PtNi alloys is reported. By tracking the evolution of both compositions and morphologies, the outward segregation of both PtO and NiO are first observed in Pt-Ni alloys. It is speculated that the diffusion of low-coordination atoms results in the formation of an energetically favorable truncated octahedron while the outward segregation of oxides leads to the formation of NiO-Pt double shells. It is very attractive that after gently removing the NiO outer shell, the dealloyed truncated octahedral core-shell structure demonstrates a greatly enhanced ORR activity. The as-obtained truncated octahedral Pt Ni core-shell alloy presents a 3.4-folds mass-specific activity of that for unannealed sample, and its activity preserves 45.4% after 30000 potential cycles of accelerated degradation test (ADT). The peak power density of the dealloyed truncated octahedral Pt Ni core-shell alloy catalyst based membrane electrolyte assembly (MEA) reaches 679.8 mW/cm , increased by 138.4 mW/cm relative to that based on commercial Pt/C.

关键词： dealloyed Pt-Ni alloys     truncated octahedron     double-shell     thermal annealing     oxygen reduction reaction (ORR)    

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Mercury removal from flue gas using nitrate as an electron acceptor in a membrane biofilm reactor

《环境科学与工程前沿（英文）》 2022年 第16卷 第2期 doi: 10.1007/s11783-021-1454-y

摘要：

Membrane bioreactor achieved mercury removal using nitrate as an electron acceptor.

关键词： Mercury removal     Oxygen     Ferrous sulfide     Transformation of mercury     Microbial community    

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Plasma for cancer treatment: How can RONS penetrate through the cell membrane?

Annemie Bogaerts, Maksudbek Yusupov, Jamoliddin Razzokov, Jonas Van der Paal

《化学科学与工程前沿（英文）》 2019年 第13卷 第2期   页码 253-263 doi: 10.1007/s11705-018-1786-8

摘要： Plasma is gaining increasing interest for cancer treatment, but the underlying mechanisms are not yet fully understood. Using computer simulations at the molecular level, we try to gain better insight in how plasma-generated reactive oxygen and nitrogen species (RONS) can penetrate through the cell membrane. Specifically, we compare the permeability of various (hydrophilic and hydrophobic) RONS across both oxidized and non-oxidized cell membranes. We also study pore formation, and how it is hampered by higher concentrations of cholesterol in the cell membrane, and we illustrate the much higher permeability of H O through aquaporin channels. Both mechanisms may explain the selective cytotoxic effect of plasma towards cancer cells. Finally, we also discuss the synergistic effect of plasma-induced oxidation and electric fields towards pore formation.

关键词： plasma medicine     cancer treatment     computer modelling     cell membrane     reactive oxygen and nitrogen species    

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Porous ultrathin-shell microcapsules designed by microfluidics for selective permeation and stimuli-triggered

《化学科学与工程前沿（英文）》   页码 1643-1650 doi: 10.1007/s11705-022-2201-z

摘要： Microcapsules are versatile delivery vehicles and widely used in various areas. Generally, microcapsules with solid shells lack selective permeation and only exhibit a simple release mode. Here, we use ultrathin-shell water-in-oil-in-water double emulsions as templates and design porous ultrathin-shell microcapsules for selective permeation and multiple stimuli-triggered release. After preparation of double emulsions by microfluidic devices, negatively charged shellac nanoparticles dispersed in the inner water core electrostatically complex with positively charged telechelic α,ω-diamino functionalized polydimethylsiloxane polymers dissolved in the middle oil shell at the water/oil interface, thus forming a porous shell of shellac nanoparticles cross-linked by telechelic polymers. Subsequently, the double emulsions become porous microcapsules upon evaporation of the middle oil phase. The porous ultrathin-shell microcapsules exhibit excellent properties, including tunable size, selective permeation and stimuli-triggered release. Small molecules or particles can diffuse across the shell, while large molecules or particles are encapsulated in the core, and release of the encapsulated cargos can be triggered by osmotic shock or a pH change. Due to their unique performance, porous ultrathin-shell microcapsules present promising platforms for various applications, such as drug delivery.

关键词： microcapsule     emulsion     microfluidics     selective permeation     stimuli-triggered release    

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Oxygen reduction electrocatalysis: From conventional to single-atomic platinum-based catalysts for protonexchange membrane fuel cells

《能源前沿（英文）》 doi: 10.1007/s11708-023-0907-3

摘要： Platinum (Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). However, their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading reduction. Based on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts, Pt single-atom catalysts (Pt SACs) as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this paper. The design thoughts and synthesis of various isolated, alloyed, and nanoparticle-contained Pt SACs are summarized. The single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the catalysts. To advance further research and development of Pt SACs for viable implementation in PEMFCs, various technical challenges and several potential research directions are outlined.

关键词： oxygen reduction electrocatalysis     Pt single-atom catalysts     conventional Pt-based catalysts     design thoughts and synthesis     metal-support interactions    

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Anion-exchange membrane direct ethanol fuel cells: Status and perspective

T.S. Zhao, Y.S. Li, S.Y. Shen

《能源前沿（英文）》 2010年 第4卷 第4期   页码 443-458 doi: 10.1007/s11708-010-0127-5

摘要： Direct ethanol fuel cells (DEFCs) are a promising carbon-neutral and sustainable power source for portable, mobile, and stationary applications. However, conventional DEFCs that use acid proton-exchange membranes (typically Nafion type) and platinum-based catalysts exhibit low performance (i.e., the state-of-the-art peak power density is 79.5 mW/cm at 90°C). Anion-exchange membrane (AEM) DEFCs that use low-cost AEM and non-platinum catalysts have recently been demonstrated to yield a much better performance (i.e., the state-of-the-art peak power density is 160 mW/cm at 80°C). This paper provides a comprehensive review of past research on the development of AEM DEFCs, including the aspects of catalysts, AEMs, and single-cell design and performance. Current and future research challenges are identified along with potential strategies to overcome them.

关键词： fuel cell     direct ethanol fuel cells     anion-exchange membrane     ethanol oxidation reaction     oxygen reduction reaction     cell performance    

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Recent advances in cathode electrocatalysts for PEM fuel cells

Junliang ZHANG

《能源前沿（英文）》 2011年 第5卷 第2期   页码 137-148 doi: 10.1007/s11708-011-0153-y

摘要： Great progress has been made in the past two decades in the development of the electrocatalysts for proton exchange membrane fuel cells (PEMFCs). This review article is focused on recent advances made in the kinetic-activity improvement on platinum- (Pt-) based cathode electrocatalysts for the oxygen reduction reaction (ORR). The origin of the limited ORR activity of Pt catalysts is discussed, followed by a review on the development of Pt alloy catalysts, Pt monolayer catalysts, and shape- and facet-controlled Pt-alloy nanocrystal catalysts. Mechanistic understanding is reviewed as well on the factors contributing to the enhanced ORR activity of these catalysts. Finally, future directions for PEMFC catalyst research are proposed.

关键词： proton exchange membrane fuel cells (PEMFCs)     cathode electrocatalysts     platinum     oxygen reduction reaction (ORR)    

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Ionic liquid modified Pt/C electrocatalysts for cathode application in proton exchange membrane fuel

Huixin Zhang, Jinying Liang, Bangwang Xia, Yang Li, Shangfeng Du

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 695-701 doi: 10.1007/s11705-019-1838-8

摘要： The modification of Pt/C catalyst by using ionic liquids to improve their catalyst activities has been reported by many researchers, but their practical behavior in operating fuel cells is still unknown. In this work, we study the ionic liquid modified Pt/C nanoparticle catalysts within cathodes for proton exchange membrane fuel cells. The influence of the ionic liquid amount, adsorption times and dispersing solvents are investigated. The experiment results show the best performance enhancement is achieved through two-time surface modification with 2 wt-% ionic liquid solution. The mechanisms are explored with the attribution to the high oxygen solubility in the ionic liquid enabling an improved oxygen diffusion in micropores and to good hydrophobicity facilitating water expelling from the active sites in fuel cell operation.

关键词： ionic liquid     PEMFC     electrode     oxygen reduction reaction     electrocatalyst     adsorption    

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标题 作者 时间 类型 操作

ethylene-co-vinyl alcohol) molecular weight and vinyl alcohol content on morphology, antifouling, and permeationproperties of polysulfone ultrafiltration membrane: thermodynamic and formation hydrodynamic behavior

期刊论文

A CO and CO

Guoxing Chen, Marc Widenmeyer, Binjie Tang, Louise Kaeswurm, Ling Wang, Armin Feldhoff, Anke Weidenkaff

期刊论文

Highly active and durable Pd-Cu catalysts for oxygen reduction in alkaline exchange membrane fuel cells

Xiong PENG, Travis J. OMASTA, Justin M. ROLLER, William E. MUSTAIN

期刊论文

Theoretical study on Janus graphene oxide membrane for water transport

Quan Liu, Mingqiang Chen, Yangyang Mao, Gongping Liu

期刊论文

Effect of PEG additives on properties and morphologies of polyetherimide membranes prepared by phase inversion

Jian CHEN, Jiding LI, Xia ZHAN, Xiaolong HAN, Cuixian CHEN,

期刊论文

Exploration of the oxygen transport behavior in non-precious metal catalyst-based cathode catalyst layerfor proton exchange membrane fuel cells

Shiqu CHEN, Silei XIANG, Zehao TAN, Huiyuan LI, Xiaohui YAN, Jiewei YIN, Shuiyun SHEN, Junliang ZHANG

期刊论文

TiO supported IrO for anode reversal tolerance in proton exchange membrane fuel cell

期刊论文

Thermal annealing synthesis of double-shell truncated octahedral Pt-Ni alloys for oxygen reduction reactionof polymer electrolyte membrane fuel cells

Xiashuang LUO, Yangge GUO, Hongru ZHOU, Huan REN, Shuiyun SHEN, Guanghua WEI, Junliang ZHANG

期刊论文

Mercury removal from flue gas using nitrate as an electron acceptor in a membrane biofilm reactor

期刊论文

Plasma for cancer treatment: How can RONS penetrate through the cell membrane?

Annemie Bogaerts, Maksudbek Yusupov, Jamoliddin Razzokov, Jonas Van der Paal

期刊论文

Porous ultrathin-shell microcapsules designed by microfluidics for selective permeation and stimuli-triggered

期刊论文

Oxygen reduction electrocatalysis: From conventional to single-atomic platinum-based catalysts for protonexchange membrane fuel cells

期刊论文

Anion-exchange membrane direct ethanol fuel cells: Status and perspective

T.S. Zhao, Y.S. Li, S.Y. Shen

期刊论文

Recent advances in cathode electrocatalysts for PEM fuel cells

Junliang ZHANG

期刊论文

Ionic liquid modified Pt/C electrocatalysts for cathode application in proton exchange membrane fuel

Huixin Zhang, Jinying Liang, Bangwang Xia, Yang Li, Shangfeng Du

期刊论文